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Appropriate non-metallic element doping is promising to improve the intrinsic electrocatalytic oxygen reduction reaction (ORR) performance of nitrogen-doped carbon candidates, yet challenges still remain to rationally design of the catalyst configuration with kinetically favorable state. Herein, we propose the metalloid element to regulate the local electronic environment, and a novel metal-free electrocatalyst, namely, atomically dispersed Te-N2 on nitrogen-doped carbon frameworks was developed. Characterization and theoretical analyses demonstrate that the heteroatoms tellurium integrated with nitrogen-doped carbon substrate forms a Te-N covalent coordination as the active center that empowers both improved ORR kinetics and structural stability. As expected, the optimized composite of Te-N-C 900 delivers considerable electrocatalytic ORR activity in alkaline media (E1/2 = 0.871 V, 0.1 M KOH), along with encouraging durability (over 10,000 cycles with 13 mV decay), which is also responsible for Zn-air batteries operating with high uplifting peak power density and long lifespan. As a proof-of-concept, this work elucidates the key influence of heteroatom interaction of metalloid element, achieves the synthesis of Te-N2 metal-free ORR catalysts, and provides guidance for the development of high-performance metal-free ORR catalysts.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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